EP0643674B1 - Process for purifying streams - Google Patents

Process for purifying streams Download PDF

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Publication number
EP0643674B1
EP0643674B1 EP93916271A EP93916271A EP0643674B1 EP 0643674 B1 EP0643674 B1 EP 0643674B1 EP 93916271 A EP93916271 A EP 93916271A EP 93916271 A EP93916271 A EP 93916271A EP 0643674 B1 EP0643674 B1 EP 0643674B1
Authority
EP
European Patent Office
Prior art keywords
packed bed
process according
ozone
cod
activated carbon
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
EP93916271A
Other languages
German (de)
English (en)
French (fr)
Other versions
EP0643674A1 (en
Inventor
Jan Peter Campen
Blandikus Catharikus Jaspers
Joannes Petrus Kaptijn
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ECO Purification Systems BV
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ECO Purification Systems BV
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Publication date
Application filed by ECO Purification Systems BV filed Critical ECO Purification Systems BV
Publication of EP0643674A1 publication Critical patent/EP0643674A1/en
Application granted granted Critical
Publication of EP0643674B1 publication Critical patent/EP0643674B1/en
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    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F1/46114—Electrodes in particulate form or with conductive and/or non conductive particles between them
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/72—Treatment of water, waste water, or sewage by oxidation
    • C02F1/78—Treatment of water, waste water, or sewage by oxidation with ozone

Definitions

  • the invention relates to a process for purifying streams which contain organic and/or inorganic impurities, the stream to be treated being introduced into a water-containing reaction zone.
  • Dutch Patent Application 9000118 discloses a method for purifying streams which contain organic and/or inorganic impurities, in which the stream to be treated is introduced into a water-containing reaction zone to which current is supplied via one or more electrodes while a substance is supplied at the same time which, under the influence of the electric current supplied, produces radicals which react with the impurities.
  • substances of this type comprise methane, carbon monoxide, hydrogen, ammonia, oxygen, ozone and hydrogen peroxide.
  • the substance producing electrochemical radicals in the process is preferably fed to the reaction zone via a porous electrode.
  • the residence time in the reaction zone can be shortened by employing elevated temperatures, preferably in the range from 10 to 95°C. The degree of conversion and the electric energy consumption in this known method still leaves something to be desired.
  • a process and apparatus for electrochemical reactions to be used for pollution control are known from US-A-3,915,822.
  • An electrochemical cell is used wherein an electrolyte - which contains impurities or undesirable components - is treated in a reaction zone containing electrically conductive particles, e.g. carbon pellets, as well as a plurality of electrodes.
  • the conductive particles may consist of activated carbon in granular, spherical or other form.
  • the voltage is normally a DC potential gradient in the order of 0.1 to 10 Volts/cm.
  • a gas reactant such as O 3 or Cl 2 may be used.
  • a mixture of O 3 in a diluent gas can be introduced to the liquid filled bed of electrically conductive particles as fine bubbles containing ozone in an amount of 2-20 vol.X.
  • the use of a sub-stoichiometric amount of ozone or any other reactant is not suggested.
  • the object of the present invention is to overcome the abovementioned drawbacks regarding energy consumption and expensive starting materials.
  • the invention provides a process for purifying streams which contain undesirable organic and/or inorganic impurities which impurities may be converted into harmless compounds by reduction or oxidation, the stream to be treated being introduced into a water-containing reaction zone which comprises a packed bed of activated carbon to which an electrochemical potential is applied and to which ozone or hydrogen is fed at the same time.
  • COD C emical O xygen D emand
  • a theoretical C hemical H ydrogen D emand (for reducible impurities), i.e. the amount of hydrogen necessary for a complete reduction with hydrogen of the micro pollutants present in the waste water.
  • the nitrate reduction using a Pd/Cu catalyst gives the reaction: 2NO - 3 + 5H 2 ⁇ N 2 + 4H 2 O + 20H - at elevated pressure.
  • the CHD amounts 8.06 mg H 2 /l.
  • sub-stoechiometry in hydrogen arises when a lower hydrogen consumption is found than 1 kg H 2 / kg CHD.
  • the process according to the invention gives rise to a lower ozone consumption than mentioned above, that is sub-stoechiometric of less than 1 kilogram of ozone per kilogram of COD reduced. The same is valid for the hydrogen consumption and CHD degradation. Consequently, the process according to the invention is characterised in that a reactant selected from ozone and hydrogen is, at the same time, fed into the reaction zone in a sub-stoechiometric amount.
  • the residence time in the reactor is low, i.e. considerably more advantageous than the effects according to WO 90/14312 and NL 9000118. It is a matter of a synergistic effect, as said effects are more favourable than the sum of the effects obtained in using the process according to said two literature references. This has been shown on the basis of experiments which will be described hereinafter.
  • a reaction zone is preferably used in which the packed bed of activated carbon consists of particles having a surface of at least 50 m 2 /g, preferably 200-1200 m 2 /g and a pore volume of at least 0.05 cm 3 /g, preferably 0.1-0.3 cm 3 /g.
  • an embodiment is used according to the invention in which the electrochemical potential of the packed bed is less than 10 volts with respect to an Hg/HgSO 4 reference electrode and preferably is in the range of 0.1-4 volts.
  • the value of the electrochemical potential is less than the voltage required for the electrolysis of water, i.e. the quantitative electrolysis of water using the cell configuration in question.
  • the potential at which water electrolysis occurs depends on the electrode material and is therefore always different for each reactor. Carbon electrodes have a relatively high overpotential for the generation of hydrogen. Furthermore, if the electrode material is contaminated, it is possible for water electrolysis to occur to a slight extent even at lower potentials. Many opposing reactions exist, but the K and Na ions which are present, for example, will not be deposited as a metal on the counterelectrode but give rise to generation of hydrogen and formation of OH - . The deposition of heavy metals, on the other hand, is possible.
  • the ozone or hydrogen consumption is surprisingly low.
  • ozone is used in an amount of 0.001-0.5 kg O 3 /kg COD of the impurities to be removed, preferably 0.005-0.3 kg O 3 /kg COD and/or in which hydrogen is used in an amount of 0.001-0.5 kg H 2 /kg CHD of the impurities to be removed, preferably 0.005-0.3 kg H 2 /kg CHD.
  • the process according to the invention therefore involves a substoichiometric ozone consumption.
  • the process according to the invention is based on a totally different mechanism compared to conventional oxidations with ozone. Thanks to this special mechanism, the process according to the invention is also suitable for the oxidation substances which cannot readily be decomposed, such as chlorinated hydrocarbons, for example freons. In the latter case carbonates, chlorides and/or fluorides are produced. Ammonia can be decomposed to give the harmless nitrogen gas.
  • the process according to the invention preferably employs a temperature in the reaction zone of at least 20°C, preferably 30-80°C. This is remarkable because, in the case of the conventional decomposition processes using ozone, there is the effect of the considerably reduced solubility of ozone gas in water at elevated temperature. In the conventional processes, therefore, an elevated pressure is used preferably (in order to accelerate the decomposition processes), which has the effect of increasing the cost of the installation. In the process according to the invention, the use of elevated pressure is unnecessary or necessary only to a small degree.
  • This apparatus comprises at least a reaction vessel containing a packed bed of activated carbon which can be operated as an electrode, a contact electrode placed in the packed bed, for the supply or removal of an electric current, a counterelectrode disposed in the reaction vessel, means for electronically insulating the packed bed of activated carbon and the counterelectrode, means for feeding in liquid, means for discharging liquid, means for feeding in ozone-containing gas, means for discharging waste gas.
  • Said means for electronic insulation may be perforated tubes or semipermeable membranes.
  • the electrodes are preferably arranged so as to be detachable, so that any deposits, for example of metals, can be removed therefrom.
  • This conventional process fails because of a still excessive COD value and in absolute terms it consumes an extraordinarily large amount of ozone, given the high COD contents.
  • Both the hydrogen consumption and the consumption of electrical charge are less than the expected stoechiometric amounts of 1 g H 2 /g CHD and 26.8 kAh/kg CHD.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Hydrology & Water Resources (AREA)
  • Engineering & Computer Science (AREA)
  • Environmental & Geological Engineering (AREA)
  • Water Supply & Treatment (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Treatment Of Water By Oxidation Or Reduction (AREA)
  • Water Treatment By Electricity Or Magnetism (AREA)
  • Water Treatment By Sorption (AREA)
  • Physical Water Treatments (AREA)
  • Separation Using Semi-Permeable Membranes (AREA)
  • Solid-Sorbent Or Filter-Aiding Compositions (AREA)
  • Treatment Of Water By Ion Exchange (AREA)
  • Cleaning By Liquid Or Steam (AREA)
  • Transition And Organic Metals Composition Catalysts For Addition Polymerization (AREA)
  • Vaporization, Distillation, Condensation, Sublimation, And Cold Traps (AREA)
EP93916271A 1992-06-04 1993-06-04 Process for purifying streams Expired - Lifetime EP0643674B1 (en)

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
NL9200989A NL9200989A (nl) 1992-06-04 1992-06-04 Werkwijze en inrichting voor het zuiveren van stromen.
NL9200989 1992-06-04
PCT/NL1993/000119 WO1993025481A1 (en) 1992-06-04 1993-06-04 Process and apparatus for purifying streams
CN93120587A CN1103385A (zh) 1992-06-04 1993-11-30 净化水的方法及装置

Publications (2)

Publication Number Publication Date
EP0643674A1 EP0643674A1 (en) 1995-03-22
EP0643674B1 true EP0643674B1 (en) 1996-09-11

Family

ID=36933440

Family Applications (1)

Application Number Title Priority Date Filing Date
EP93916271A Expired - Lifetime EP0643674B1 (en) 1992-06-04 1993-06-04 Process for purifying streams

Country Status (24)

Country Link
US (1) US5565107A (cs)
EP (1) EP0643674B1 (cs)
JP (1) JP2748047B2 (cs)
CN (1) CN1103385A (cs)
AT (1) ATE142607T1 (cs)
AU (1) AU668747B2 (cs)
BR (1) BR9306478A (cs)
CA (1) CA2136869A1 (cs)
CZ (1) CZ284039B6 (cs)
DE (1) DE69304699T2 (cs)
DK (1) DK0643674T3 (cs)
ES (1) ES2092320T3 (cs)
FI (1) FI945689A7 (cs)
GR (1) GR3021345T3 (cs)
HK (1) HK134397A (cs)
HU (1) HUT68766A (cs)
NL (1) NL9200989A (cs)
NO (1) NO944657L (cs)
NZ (1) NZ254248A (cs)
RO (1) RO113028B1 (cs)
RU (1) RU2088538C1 (cs)
SK (1) SK147794A3 (cs)
TJ (1) TJ190R3 (cs)
WO (1) WO1993025481A1 (cs)

Families Citing this family (21)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB9408124D0 (en) * 1994-04-23 1994-06-15 Univ Waterloo Electrically-enhanced degradation of organic contaminants using zero-valent metals
GB9603741D0 (en) * 1996-02-22 1996-04-24 Lin Mei Treatment of water by electrolysis
US5879555A (en) * 1997-02-21 1999-03-09 Mockba Corporation Electrochemical treatment of materials
JP3662111B2 (ja) * 1997-06-24 2005-06-22 アルプス電気株式会社 洗浄液の製造方法およびそのための装置
FR2783515B1 (fr) * 1998-09-21 2000-12-15 Conservatoire Nat Arts Procede de traitement de substances organiques en milieu aqueux, notamment d'effluents et dispositif electrochimique pour mettre en oeuvre le procede
US6298996B1 (en) * 1999-02-05 2001-10-09 Eltron Research, Inc. Three dimensional electrode for the electrolytic removal of contaminants from aqueous waste streams
WO2000048945A1 (de) * 1999-02-19 2000-08-24 Winfried Schellbach Vorrichtung zur elektrokatalytischen behandlung von mit schadstoffen und/oder mikroorganismen belasteten flüssigkeiten
DE19911875A1 (de) * 1999-03-17 2000-09-28 Judo Wasseraufbereitung Vorrichtung zur elektrolytischen Behandlung von Wasser bzw. wässrigen Lösungen
US6197177B1 (en) * 1999-11-06 2001-03-06 Silkroad Corp. Water treating apparatus with electro-chemistry process
GB2367072A (en) * 2000-03-22 2002-03-27 Univ Brunel Mineraliser reaction cell for purifying liquids
JP3990993B2 (ja) * 2003-02-10 2007-10-17 恒久 荒磯 難分解性有機化合物の分解方法およびその装置
RU2286950C2 (ru) * 2003-02-28 2006-11-10 Алексей Юрьевич Кочетков Способ электрокаталитической очистки питьевых и сточных вод
US7309408B2 (en) * 2003-06-11 2007-12-18 Alfonso Gerardo Benavides Industrial wastewater treatment and metals recovery apparatus
RU2247078C1 (ru) * 2003-06-24 2005-02-27 ФГУП ГНЦ РФ Научно-исследовательский физико-химический институт им. Л.Я. Карпова Способ обработки вод (варианты)
ES2265728B1 (es) * 2004-09-10 2008-02-01 Universidad De Granada Sistema de eliminacion de microcontaminantes organicos de las aguas mediante el uso de ozono y carbon activado.
CZ297103B6 (cs) 2004-10-06 2006-09-13 Lysytchuk@Oleg Zpusob cistení tekutin za pouzití ionizacního provzdusnování
US7967967B2 (en) * 2007-01-16 2011-06-28 Tesla Laboratories, LLC Apparatus and method for electrochemical modification of liquid streams
CN102001740A (zh) * 2010-07-29 2011-04-06 攀钢集团冶金工程技术有限公司 处理钢铁冶炼废水的方法
WO2012076940A1 (en) * 2010-12-06 2012-06-14 Council Of Scientific & Industrial Research Carbon bed electrolyser for treatment of liquid effluents and a process thereof
CN103318990B (zh) * 2013-07-04 2014-10-08 哈尔滨工业大学 电化学阴极催化臭氧氧化去除水中有机污染物的方法
RU168902U1 (ru) * 2016-10-11 2017-02-27 Федеральное государственное бюджетное образовательное учреждение высшего образования "Уфимский государственный нефтяной технический университет" Фильтр для очистки воды

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Publication number Priority date Publication date Assignee Title
US3793173A (en) * 1969-02-03 1974-02-19 K Price Wastewater treatment using electrolysis with activated carbon cathode
US3730885A (en) * 1971-01-21 1973-05-01 Tvco Lab Inc Electrochemical control of adsorption and desorption with activated carbon
DE2424091C3 (de) * 1974-05-17 1980-11-27 Sachs Systemtechnik Gmbh, 8720 Schweinfurt Verfahren zur anodischen Oxidation organischer Belastungsstoffe im Wasser in einer Wirbelschicht aus leitfähigem Adsorbens
US3915822A (en) * 1974-05-22 1975-10-28 Grace W R & Co Electrochemical system with bed sections having variable gradient
US4072596A (en) * 1975-04-30 1978-02-07 Westinghouse Electric Corporation Apparatus for removal of contaminants from water
CH633497A5 (de) * 1977-03-30 1982-12-15 Kernforschungsanlage Juelich Verfahren zur reduktion von reduzierbaren schadstoffen in waessrigen loesungen.
US4351734A (en) * 1977-05-02 1982-09-28 Ametek, Inc. Spark cell ozone generator
US4130483A (en) * 1977-10-14 1978-12-19 Nuclear Supreme Sewage treating and conversion process
US4260484A (en) * 1979-03-29 1981-04-07 Standard Oil Company (Indiana) Process for renewing the adsorptive capacity of a bed of active carbon
DE3430485A1 (de) * 1984-08-18 1986-02-27 Basf Ag, 6700 Ludwigshafen Brennstoffzelle
US4954469A (en) * 1988-08-01 1990-09-04 Robinson Ken K Granulated activated carbon for water treatment
US4983267A (en) * 1988-10-18 1991-01-08 Innova/Pure Water, Inc. Water deionization and contaminants removal or degradation
WO2014045556A1 (ja) 2012-09-18 2014-03-27 日本電気株式会社 時系列データ処理装置、時系列データ処理方法及び時系列データ処理プログラムの記憶媒体

Also Published As

Publication number Publication date
WO1993025481A1 (en) 1993-12-23
DE69304699D1 (de) 1996-10-17
SK147794A3 (en) 1995-06-07
BR9306478A (pt) 1998-01-13
EP0643674A1 (en) 1995-03-22
DE69304699T2 (de) 1997-03-06
CA2136869A1 (en) 1993-12-23
NL9200989A (nl) 1994-01-03
HUT68766A (en) 1995-07-28
AU668747B2 (en) 1996-05-16
CN1103385A (zh) 1995-06-07
FI945689A0 (fi) 1994-12-02
GR3021345T3 (en) 1997-01-31
FI945689A7 (fi) 1994-12-02
CZ303394A3 (en) 1995-03-15
NZ254248A (en) 1996-08-27
RO113028B1 (ro) 1998-03-30
AU4587793A (en) 1994-01-04
DK0643674T3 (da) 1996-09-30
RU2088538C1 (ru) 1997-08-27
NO944657D0 (no) 1994-12-02
ES2092320T3 (es) 1996-11-16
US5565107A (en) 1996-10-15
JP2748047B2 (ja) 1998-05-06
TJ190R3 (en) 1998-10-28
CZ284039B6 (cs) 1998-07-15
NO944657L (no) 1994-12-02
RU94046244A (ru) 1996-12-20
JPH07507491A (ja) 1995-08-24
HK134397A (en) 1998-02-27
HU9403477D0 (en) 1995-02-28
ATE142607T1 (de) 1996-09-15

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